Donor engineering of a benzothiadiazole-based D-A-D-type molecular semiconductor for perovskite solar cells: a theoretical study.

Due to the easy formation of compact molecular packing arrangements and the favorable photophysical and electrochemical properties, donor-acceptor-donor (D-A-D)-type small molecule hole-transporting materials (HTMs) have been widely synthesized and researched to improve the efficiency and stability of perovskite solar cells (PSCs). The main approach in recent experiments has been to seek good acceptors, whereas the influence of the electron-donating units has been less reported. In this work, six new benzothiadiazole-based D-A-D-type HTMs are tailored by employing the ethyl-substituted phenoxazine (POZ), phenothiazine (PTZ) and carbazole (CZ) as the donors.

Buried Interface Regulation by Bio-Functional Molecules for Efficient and Stable Planar Perovskite Solar Cells.

Among the factors that lead to the reduction of the efficiency of perovskite solar cells (PSCs) the difficulty involved in realizing a high-quality film and the efficient charge transfer that takes place at the interface between electron-transport layer (ETL) and perovskite is worth mentioning. Here, a strategy for planar-type devices by natural bio-functional interfaces that uses a buried electron-transport layer made of cobalamin complexed tin oxide (SnO @B ) is demonstrated. Having systematically investigated the effects of SnO @B interfacial layer in perovskite solar cells, it can be concluded that cobalamin can chemically link the SnO layer and the perovskite layer, resulting in improved perovskite film quality and interfacial defect passivation.

Tailoring of the core structure towards promising small molecule hole-transporting materials for perovskite solar cells: a theoretical study.

The design of new molecules with theoretical chemistry methods and further obtaining a fundamental understanding of the structure-property relationship are important for the development of high-efficiency hole-transporting materials (HTMs). Herein, the effect of semi-locked and fully-locked cores was systematically investigated based on two conformation-tunable tetrathienylethene (TTE) and tetraphenylethylene (TPE) units. Our results show that the highest occupied molecular orbital (HOMO) levels of the locked TTE-2 and TTE-3 are clearly down-shifted compared with that of the unlocked TTE-1, which is due to the decreased electronic conjugation between the locked cores and the triphenylamine (TPA) arms, whereas the same situation is not found for TPE-3 due to the twisted core configuration.

Boosting the hole transport of conductive polymers by regulating the ion ratio in ionic liquid additives.

Poly(3,4-ethylenedioxythiophene) (PEDOT) has aroused great interest in organic electrics because of its high electrical conductivity and mechanical flexibility. To improve the charge transport, it can act as an ionic liquid (IL) additive due to its ion characteristics and high electrical conductivity. Herein, we investigated the hole-transport performance of PEDOT treated by ILs featuring specific ion ratios (4 : 1, 3 : 1, 2 : 1, 1 : 1, 1 : 2, 1 : 3, and 1 : 4) of the cation and anion through classical dynamics simulations and quantum mechanics computations.

Understanding the effects of the co-sensitizing ratio on the surface potential, electron injection efficiency, and Förster resonance energy transfer.

Multiple absorbers that function in different absorption regions (near infra-red (NIR) and UV-Visible (UV-Vis)) have been widely used in solar cell applications to enhance the light-harvesting. Herein, two special co-sensitizing Models 1 and 2, which feature either saturated dye IQ21 or saturated co-sensitizer S2, have been added to a TiO surface to explore the effect of the altered sensitizing sequence, namely the co-sensitizing ratio of IQ21/S2 and S2/IQ21 on the electrostatic potential variation (ΔV), electron injection efficiency (η'), and Förster resonance energy transfer (FRET), using density functional theory and first-principle molecular dynamics simulations. The ΔV related to the open-circuit voltage (V) is insensitive in both Models 1 and 2.

Probing effects of molecular conformation on the electronic and charge transport properties in two- and three-dimensional small molecule hole-transporting materials: a theoretical investigation.

Thiophene/benzene-fused π-conjugated systems are normally employed as the core units of two- and three-dimensionally expanded small molecule hole-transporting materials (HTMs) to improve their electronic and charge transport properties, whereas comparison studies between two-dimensional and three-dimensional core conformations are less reported. To further find useful clues for the design of highly-efficient small molecule HTMs and to find new core units, in this work, four HTM molecules are designed by employing triphenylene, benzotrithiophene, triptycene, and thiophenetriptycene as the core units, and simulated with density functional theory combined with the Marcus hopping model. Our results show that all the considered HTMs display appropriate molecular energy levels, less optical absorption in the visible light region and large Stokes shifts, and high hole mobilities (9.

How to design more efficient hole-transporting materials for perovskite solar cells? Rational tailoring of the triphenylamine-based electron donor.

Designed with a symmetrical naphthatetrathiophene (NTT) core and triphenylamine (TPA)-based side arms, a series of novel organic small molecule hole-transporting materials are simulated for perovskite solar cells (PSCs) using density functional theory (DFT) and time-dependent DFT (TD-DFT) methods. As a fundamental understanding, the energy level alignments and the charge transport behavior are explored for their potential applications. Our results show that, adding an oxygen-bridge between the neighboring phenyl groups of TPA side arms makes the highest occupied molecular orbital (HOMO) levels up-shift, whereas the carbon-carbon single bond stabilizes the HOMOs by about 0.

Nanoscale Structural Modulation and Low-temperature Magnetic Response in Mixed-layer Aurivillius-type Oxides.

Nanoscale structural modulation with different layer numbers in layer-structured complex oxides of the binary BiTiO-BiFeO system can give rise to intriguing phenomena and extraordinary properties, originating from the correlated interfaces of two different phases with different strain states. In this work, we studied the nanoscale structural modulation induced by Co-substitution in the Aurivillius-type oxide of BiFeTiO with a unique and naturally occurred mixed-layer structure. Nanoscale structural evolution via doping occurred from the phase-modulated structure composed of 4- and 5-layer phases to a homogeneous 4-layer structure was clearly observed utilizing x-ray diffraction and electron micro-techniques.

Additive-Enhanced Crystallization of Solution Process for Planar Perovskite Solar Cells with Efficiency Exceeding 19 .

To reduce intrinsic defect density in perovskite films, various additives are often added into the precursor solution. In this paper, a novel solution, in which isopropanol (IPA) was added into the precursor solution, was developed for the preparation of normal planar perovskite solar cells (PSCs). A champion power conversion efficiency (PCE) of 19.

The electron injection rate in CdSe quantum dot sensitized solar cells: from a bifunctional linker and zinc oxide morphology.

Herein, we have investigated the effect of both the bifunctional linker (L1, L2, L3, and L4) and ZnO morphology (porous nanoparticles (NPs), nanowires (NWs), and nanotubes (NTs-A and NTs-Z)) on the electron injection in CdSe QD sensitized solar cells by first-principles simulation. Via calculating the partitioned interfaces formed by different components (linker/QDs and ZnO/linker), we found that the electronic states of QDs and every ZnO substrate are insensitive to any linker, while the frontier orbitals of L1-L4 (with increased delocalization) manifest a systematical negative-shift. Because of the lowest unoccupied molecular orbital (LUMO) of L1 compared to its counterparts aligned in the region of the virtual states of QDs or the substrate with a high density of states, it always yields a stronger electronic coupling with QDs and varied substrates.

Theoretical investigation on structural and electronic properties of organic dye C258 on TiO₂(101) surface in dye-sensitized solar cells.

The structural and electronic properties of an organic dye C258 before and after being adsorbed onto a TiO2(101) surface by two adsorption modes, monodentate (Mha) and bidentate bridging (BBH), have been investigated in detail. The combination of density functional tight-binding (DFTB), density functional theory (DFT), and time-dependent DFT (TDDFT) approaches have been employed. DFT calculations show that C258 has remarkable charge-transfer characteristics, which favors fast electron injection from the excited dye to the conduction band of TiO2.

Iodinated Al(III)-based phthalocyanines are promising sensitizers for dye-sensitized solar cells; a theoretical comparison between Zn(II), Mg(II), and Al(III)-based phthalocyanine sensitizers.

To design efficient dyes for dye-sensitized solar cells (DSSCs), using a Zn-coordinated phthalocyanine (TT7) as the prototype, a series of phthalocyanine dyes (Pcs) with different metal ions and peripheral/axial groups have been investigated by means of density functional theory (DFT) and time-dependent DFT (TDDFT) methods. Computational results show that the iodinated Al-based dye with a peripheral amino group (Al-I-NH2-Pc) exhibits the largest redshift in the maximum absorbance (λ(max)). In addition, Al-based dyes have appropriate energy-level arrangements of frontier orbitals to keep excellent balance between electron injection and regeneration of oxidized dyes.